Frontiers in Chemistry
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2022
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IF 5.545
Qian Ningkang,Ji Liang,Li Xiao,Huang Jingbo,Li Junjie,Wu Xingqiao,Yang Deren,Zhang Hui
Combining the core-shell structure with the optimization of surface composition and structure in the shell is a fantastic strategy to enhance the electrocatalytic performances. Here, we synthesized trimetallic Au@PtxSny core-shell nanoparticles (NPs) with tunable composition and structure of Pt-Sn alloyed shells. Impressively, the Au@PtSn core-shell NPs with hexagonal PtSn alloyed shells exhibited the highest mass activity and specific activity toward ethanol oxidation reaction (EOR) in alkaline electrolyte, which are 13.0 and 12.7 times higher than those of the commercial Pt/C. In addition, the Au@PtSn core-shell NPs displayed the best stability compared to commercial Pt/C, with only 44.8% loss vs. 86.8% loss in mass activity after 1,000 s due to the stronger anti-poisoning ability for reaction intermediates. The theory calculations reveal that the introduction of Au core and alloying Pt with Sn both endow Pt with an appropriate d-band center, and thus effectively boosting the EOR activity.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Tianle Shi,Yong Men,Shuang Liu,Jinguo Wang,Zhuping Li,Keye Qin,Dandan Tian,Wei An,Xiaoli Pan,Lin Li
Hydrogenation of CO 2 to methanol is an achievable way for “methanol economy” and “liquid sunshine” visions. Owing to highly tunable properties containing different morphologies, exposed crystal facets and oxygen vacancies , In 2 O 3 has become a promising material for CO 2 hydrogenation. Here we successfully introduced highly dispersed Pt 2+ species into three different morphologies In 2 O 3 supports by controllable precipitation method. The dominant exposed crystal facets of In 2 O 3 supports during the research are discovered to greatly affect the dispersion of active Pt 2+ species and the number of oxygen vacancies, as analyzed by diverse characterization techniques, and closely correlated with the catalytic performance. Compared with Pt/In 2 O 3 whcih mainly exposing (222) or (104) facet, Pt/In 2 O 3 which primarily exposed (211) facet obtained higher catalytic activity, including a CO 2 conversion of 11.7% and methanol selectivity of 74.8% with a space time yield of methanol of 0.63 g MeOH h −1 gcat −1 at 300 °C, 5 MPa, and 21,000 cm 3 h −1 g −1 . The highly enhanced activity of 1.5Pt/C-In 2 O 3 -S catalyst was ascribed to its more abundant oxygen vacancies and well-dispersed Pt 2+ species, which derived from the interaction between Pt 2+ and the underlying In 2 O 3 (211) facet. The special interface structure enabled the activation of CO 2 and hydrogenation of key intermediates effectively. Exposing the highly active crystal face of the In 2 O 3 supports is proved to be an effective strategy to enhance catalytic performance of Pt/In 2 O 3 catalyst for methanol synthesis .
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Kailin Wang,Songyu Yang,Yan Wu
Dual cocatalysts play an important role in photocatalytic water splitting to hydrogen production . In this paper, Fe-doped Co 3 O 4 (Fe-Co 3 O 4 ) and Pt were loaded on the surface of g -C 3 N 4 to enhance the water photocatalytic splitting, in which Fe-Co 3 O 4 was used as an oxidation cocatalyst to capture the photo-generated holes of g -C 3 N 4 , and Pt was used as a reduction cocatalyst to transfer photo-generated electrons. Under the irradiation of visible light, its hydrogen production rate reaches up to 3.015 mmol g −1 h −1 , which is 3.01 times higher than that of g -C 3 N 4 loaded with Pt. Pt and Fe-Co 3 O 4 dual cocatalysts not only promote the migration rate of photo-generated electrons and holes on the surface of g -C 3 N 4 , but also improve the light absorption capacity of visible light. The interfacial electric field built from the p-n heterojunction of Fe-Co 3 O 4 / g -C 3 N 4 drives photo-generated electrons in Fe-Co 3 O 4 flowing to the holes of g -C 3 N 4 , which further inhibiting the recombination of g -C 3 N 4 photo-generated carriers. This work provides a reference for the development of high-efficiency photocatalyst and an effective support for the development of semiconductor cocatalyst.
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Nanomaterials
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2022
·Vol. 12
·期 15
·2550
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IF 5.719
Yuqian Yu,Li Kang,Lixian Sun,Fen Xu,Hongge Pan,Zhen Sang,Chenchen Zhang,Xinlei Jia,Qingli Sui,Yiting Bu,Dan Cai,Yongpeng Xia,Kexiang Zhang,Bin Li
Sodium borohydride (NaBH4), with a high theoretical hydrogen content (10.8 wt%) and safe characteristics, has been widely employed to produce hydrogen based on hydrolysis reactions. In this work, a porous titanium oxide cage (PTOC) has been synthesized by a one-step hydrothermal method using NH2-MIL-125 as the template and L-alanine as the coordination agent. Due to the evenly distributed PtNi alloy particles with more catalytically active sites, and the synergistic effect between the PTOC and PtNi alloy particles, the PtNi/PTOC catalyst presents a high hydrogen generation rate (10,164.3 mL∙min−1∙g−1) and low activation energy (28.7 kJ∙mol−1). Furthermore, the robust porous structure of PTOC effectively suppresses the agglomeration issue; thus, the PtNi/PTOC catalyst retains 87.8% of the initial catalytic activity after eight cycles. These results indicate that the PtNi/PTOC catalyst has broad applications for the hydrolysis of borohydride.Keywords:hydrogen generation;porous titanium oxide cage;PtNi nanoparticles;sodium borohydride hydrolysis
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ACS Applied Nano Materials
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2022
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IF 6.14
Yujia Yuan,Zhongliang Huang,Siyuan Hu,Dongren Cai,Guowu Zhan
In the field of catalysis, nanoreactors with spatially restricted effects play a critical role to enhance the production efficiency of a variety of reactions. In this contribution, we used ZIF-67 nanocubes (size of 140 nm) as a template and conformally deposited Al2O3 thin films by the atomic layer deposition (ALD) technique, wherein Pt nanoparticles (Pt NPs) as active sites were loaded on either the inside or outside of the Al2O3 films. Notably, it was found that the water treatment of the nanoreactors was critical to the enhanced catalytic CO oxidation performance with substantially decreased T100 (temperature to achieve 100% conversion). Various characterization results indicated the successful synthesis of yolk–shell structured ZIF-67/Pt@10Al2O3-W catalyst with excellent CO oxidation activity and good long-term stability. In addition, in situ diffuse reflectance infrared Fourier transform spectroscopy was used to explore the catalytic oxidation process, and the results revealed that the reason for the superior CO catalytic activity of the designed nanoreactors was ascribed to the moderate CO surface coverage provided by the Al2O3 films and the activated oxygen species. In summary, this work provides some insights into the preparation of metal–organic framework-based nanoreactors using ALD-assisted methods.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Ya Zhang,Lang Hu,Yongcai Zhang,Xiaozhi Wang,Honggui Wang
Snowflake-like Cu 2 S/MoS 2 heterostructures with varied compositions were constructed via a two-step hydrothermal method. The 45-Cu 2 S/MoS 2 with 45 wt% Cu 2 S was found as the optimum catalyst, which displayed photothermal enhanced hydrogen evolution reaction (HER) performance under near infrared (NIR) irradiation. After electrochemical deposition of a tiny amount of Pt (45-Cu 2 S/MoS 2 /Pt-100s), Schottky barrier was formed between Pt nanoparticles and MoS 2 nanosheets . Using 45-Cu 2 S/MoS 2 /Pt-100s as an electrocatalyst, low overpotential of 78 mV (@10 mV cm −2 ) and Tafel slope of 48 mV dec −1 were achieved with the assistance of NIR irradiation. The photoelectrochemical (PEC) hydrogen production performance of 45-Cu 2 S/MoS 2 /Pt-100s was also investigated. The optimal conversion efficiency of 45-Cu 2 S/MoS 2 /Pt-100s could reach 0.78% at 0.57 V (vs. reversible hydrogen electrode (RHE)). The control of the internal geometric and electronic structure of the catalysts and the aid of photothermal effect in this work provide new ideas for designing high-efficiency hydrogen evolution catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Xing Cheng,Yueshuai Wang,Yue Lu,Lirong Zheng,Shaorui Sun,Hongyi Li,Ge Chen,Jiujun Zhang
Reducing the usage of noble metals, such as platinum-based catalysts for oxygen reduction reaction (ORR) is pressingly demanded towards the practical applications of proton-exchange membrane fuel cells. One promising way is to develop Pt single atom catalysts (SACs), which, however, are plagued by their preference toward two-electron ORR pathway as well as stability issue. Herein, a single-atom alloy (SAA) catalyst with platinum-cobalt (Pt-Co) dual sites encapsulated in nitrogen-doped graphitized carbon nanotubes (Pt 1 Co 100 /N-GCNT) consisting of isolated Pt atoms decorated on the surface of Co nanoparticles was reported. Based on complementary spectroscopic characterizations and first-principle calculations, we propose that the unique Pt-Co dual sites in SAA facilitates the adsorption and dissociation of oxygen, particularly for the immobilization of OOH* intermediate and the dissociation of OH* intermediate, and thus result in high-efficiency four-electron ORR pathway. Consequently, the Pt 1 Co 100 /N-GCNT SAA catalyst achieves a mass activity of 0.81 A mg –1 Pt at 0.90 V (versus the reversible hydrogen electrode) in 0.1 M HClO 4 electrolyte, outperform commercial Pt/C catalyst for 5.4 times. The superior stability of the SAA catalyst was reflected by the results from the 30,000 potential-scanning cycles combined with the post characterization of the catalyst.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Yuyun Ye,Hongli Yu,Bohan Chen,Yifan Zhao,Bai Lv,Guanghe Xue,Yong Sun,Jie Cao
Photodynamic therapy (PDT), as a promising strategy in cancer treatment that utilizes photosensitizers (PSs) to produce reactive oxygen species, has been widely used for eliminating cancer cells under specific wavelength light irradiation. However, the low aqueous solubility of PSs and special tumor microenvironments (TME), such as high glutathione (GSH) and tumor hypoxia remain challenges towards PDT for hypoxic tumor treatment. To address these problems, we constructed a novel nanoenzyme for enhanced PDT-ferroptosis therapy by integrating small Pt nanoparticles (Pt NPs) and near-infrared photosensitizer CyI into iron-based metal organic frameworks (MOFs). In addition, hyaluronic acid was adhered to the surface of the nanoenzymes to enhance the targeting ability. In this design, MOFs act not only as a delivery vector for PSs, but also a ferroptosis inducer. Pt NPs stabilized by MOFs were functioned as an oxygen (O 2 ) generator by catalyzing hydrogen peroxide into O 2 to relieve tumor hypoxia and increase singlet oxygen generation. In vitro and in vivo results demonstrated that under laser irradiation, this nanoenzyme could effectively relive the tumor hypoxia and decrease the level of GSH, resulting in enhanced PDT-ferroptosis therapy against hypoxic tumor. The proposed nanoenzymes represent an important advance in altering TME for improved clinical PDT-ferroptosis therapy, as well as their potential as effective theranostic agents for hypoxic tumors.
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Molecular Catalysis
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2023
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IF 4.6
Xiqiang Tian,Yanping Dong,Muhammad Zahid
Herein, WN-TiO 2 with evenly distributed WN nanoparticles (NPs) were facilely synthesized thru one pot evaporation-induced self-assembly (EISA) and nitridation treatment method, as an active host material for precious Pt NPs. A number of characterization techniques were executed to explore the influence of the synthetic approach upon the surface and catalytic properties of the as-synthesized 2wt%Pt/TiO 2 and 2wt%Pt/WN-TiO 2 catalysts. As compared to 2wt%Pt/TiO 2 , the 2wt%Pt/WN-TiO 2 catalyst exhibited outstanding performance in the selective hydrogenation reaction of Furfural (FAL) to Furfuryl alcohols (FOL) (conversion (97.8%) and selectivity (98.6%)). The 2wt%Pt/WN-TiO 2 catalyst also exhibited an impressive recyclability performance for up to five recycles without significant deactivation in activity and selectivity. The superior catalytic hydrogenation performance can be ascribed to the specific nanostructure characteristics of the catalyst arose from the possible synergistic effect occurred between Pt and WN species of 2wt%Pt/WN-TiO 2 . Besides, the improved homogeneous dispersion of precious Pt NPs causes more exposed active sites of Pt 0 species on the surface of 2wt%Pt/WN-TiO 2 , which is very beneficial for the improved hydrogenation of FAL to FOL.
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RSC Advances
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2023
·Vol. 13
·期 20
·13556-13563
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IF 3.9
Xia Xu,Mingqiang Li,Liming Yang,Bing Hu
Reasonable design of bimetallic nanomaterials with support is beneficial to improve catalytic performance. This work reports a new kind of sodium sesquicarbonate-supporting Fe2O3@Pt via etching Fe3O4@Pt@SiO2, which exhibits highly efficient and stable catalytic reduction performance towards 4-NP. Sodium sesquicarbonate-supporting Fe2O3@Pt has an interconnected one-dimensional network structure that provides sufficient channels for mass transfer. At the same time, a large amount of Fe2O3@Pt is exposed on its surface, which hinders the aggregation of pt clusters and Fe2O3 nanoparticles, and facilitates the direct contact of Fe2O3@Pt reaction sites with reactant molecules, thus improving the catalytic rate of 4-NP reduction reaction. Moreover, the introduction of non-metallic Fe can not only reduce the consumption of precious metal Pt, but also improve the catalytic efficiency due to the synergistic effect. This study opens up a new avenue to develop robust catalysts for heterogeneous catalytic reactions.
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JOURNAL OF CATALYSIS
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2023
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IF 7.3
Darong He,Xinmei Ding,Shanshan Li,Yaxin Liu,Ming Zhao,Jianli Wang,Yaoqiang Chen
Deep catalytic removal of nitrogen oxides is one of the widespread research topics, mainly limited by the low temperature activity and hydrothermal stability of the first step for NO oxidation. Oxygen vacancies (O v ) and oxygen migration capacity play a crucial role in this challenge. Particularly, tuning the Mn-O coordination environment according to the radius and valence differences of dopant ions can increase O v , while accelerate oxygen migration by constructing Pt/mullite interfaces. Here, based on the hydrothermal stability of Pt/mullite to NO oxidation, we designed Mg 2+ - and Ba 2+ -doped catalysts. And the NO oxidation performance of the Mg 2+ -doped catalyst was significantly enhanced compared to the undoped catalysts (After hydrothermal aging, turnover frequency = 1.9 s −1 at 150 °C and activation energy = 21 kJ/mol). Meanwhile, all catalysts tested with simulated diesel exhaust and the NO oxidation performance showed essentially no decrease after 16 h of hydrothermal aging at 800 °C. Furthermore, X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR) demonstrated the O v content of doped catalysts increased significantly. In addition, O 2 temperature programmed desorption (O 2 -TPD) and Thermogravimetry (TG) proved that the oxygen migration capacity of doped catalysts was enhanced by several times. Notably, the simple doping method is general for the modification of other mullites and worthy of industrial application.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Yunqi Yu,Jianting He,Tong Wang,Xinsheng Qiu,Kangcheng Chen,Qin Wu,Daxin Shi,Yaoyuan Zhang,Hansheng Li
Nitrogen-doped carbon nanotubes (N-CNTs) prepared by carbonization of polypyrrole nanotubes (PPy-NTs) are used as supports. Pt–CeO 2 /N-CNTs electrocatalysts are successfully prepared by in-situ growth of Pt and CeO 2 nanoparticles (NPs) via a one-step coupling method of co-deposition and ethylene glycol reduction. Through structural characterization and electrochemical tests of the prepared electrocatalysts, the effects of preparation conditions on the structure of the electrocatalysts and their electrocatalytic activity for methanol oxidation were systematically investigated. The results verify that the Pt–CeO 2 /N-CNTs electrocatalysts were prepared using N-CNTs calcined at 700 °C as a support and 15 mM alkali concentration. They have the largest electrochemical active area and methanol oxidation mass activity of 85 m 2 g −1 (Pt) and 722 A g −1 (Pt), respectively. Furthermore, the electrochemical stability and anti-CO poisoning performance of the electrocatalysts are significantly better than those of the commercial Pt/C electrocatalysts. The highly-dispersed Pt and CeO 2 in Pt–CeO 2 /N-CNTs, a large number of N sites, and the synergistic action of Pt, CeO 2 , and N-CNTs result in a catalyst with excellent electrocatalytic activity, stability, and resistance to CO poisoning. The support structure and the dispersion of Pt and CeO 2 can be controlled by changing the preparation conditions, which provides a basis for the industrial application of direct methanol fuel cells.
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